Abstract

BackgroundGlyphosate and its salt formulations are nonselective herbicides that have been extensively used worldwide, both for residential and agricultural purposes. The possible carcinogenicity and teratogenicity of glyphosate remain to be elucidated. We developed a sensitive and high-throughput analytical method for urinary glyphosate using liquid chromatography-tandem mass spectrometry with the aim of contributing to glyphosate exposure assessment in epidemiological studies.MethodsAfter urine dilution (creatinine matching dilution to 0.05 g creatinine/L), glyphosate was extracted using two types of solid phase extraction columns (SCX and NH2) with automated sample preparation instruments. The eluate was dried and dissolved in the mobile phase, followed by liquid chromatography-tandem mass spectrometry analysis. The optimized method was applied to urine samples obtained from 54 Japanese adults and children.ResultsThe results from the validation study demonstrated good recoveries (91.0-99.6%), within- and between-run precisions (< 15%), low detection limits (0.1 μg/L), and lower limit of quantification (0.3 μg/L). The detection frequency and median concentration of the urinary glyphosate in Japanese subjects were 59% and 0.25 μg/L (0.34 μg/g creatinine).ConclusionsOur reliable determination method was successful in measuring urinary glyphosate concentration. Moreover, this is the first biomonitoring report of urinary glyphosate levels in the Japanese general population.

Highlights

  • Glyphosate and its salt formulations are nonselective herbicides that have been extensively used worldwide, both for residential and agricultural purposes [1]. In countries where their use is allowed for cultivation of genetically modified glyphosate-resistant crops such as wheat and corn and in Japan and other counties, glyphosate is frequently used in agricultural fields, playgrounds, parking areas, and roads for weed control [2]

  • This study aimed to develop a fully validated quantitative method for urinary glyphosate, which is applicable to the general population with no documented exposure to glyphosate using liquid chromatography-tandem mass spectrometry (LC-Mass spectrometry (MS)/MS)

  • Optimization of the LC column and mobile phase Given that glyphosate is an ionic and highly watersoluble compound, it is difficult to hold it using a common LC separation column such as a reversed-phase column

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Summary

Introduction

Glyphosate and its salt formulations are nonselective herbicides that have been extensively used worldwide, both for residential and agricultural purposes [1]. Whether the widely used glyphosate poses a possible risk to human health is a controversial matter. Several regulatory agencies [5,6,7] reviewed the scientific data and denied the carcinogenicity of glyphosate. A largescale cohort study focused on the relationship between glyphosate exposure and health risks. The Agricultural Health Study, which is a prospective cohort study in North Carolina and Iowa, reported that a relationship was evident between glyphosate exposure and the risk of acute myeloid leukemia [8]. In view of the prospective, large-scale increase in the glyphosate usage level worldwide, nationwide studies covering exposure assessment of glyphosate followed by risk assessment are needed in Japan as well. We developed a sensitive and high-throughput analytical method for urinary glyphosate using liquid chromatography-tandem mass spectrometry with the aim of contributing to glyphosate exposure assessment in epidemiological studies

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